Coherent light pulses of few to hundreds of femtoseconds (fs) duration have prolifically served the field of ultrafast phenomena. While fs pulses address mainly dynamics of nuclear motion in molecules or lattices in the gas, liquid or condensed matte
r phase, the advent of attosecond pulses has in recent years provided direct experimental access to ultrafast electron dynamics. However, there are processes involving nuclear motion in molecules and in particular coupled electronic and nuclear motion that possess few fs or even sub-fs dynamics. In the present work we have succeeded in addressing simultaneously vibrational and electronic dynamics in molecular Hydrogen. Utilizing a broadband extreme-ultraviolet (XUV) continuum the entire, Frank-Condon allowed spectrum of H2 is coherently excited. Vibrational, electronic and ionization 1fs scale dynamics are subsequently tracked by means of XUV-pump-XUV-probe measurements. These reflect the intrinsic molecular behavior as the XUV probe pulse hardly distorts the molecular potential.
Studies of ultrafast dynamics along with femtosecond-pulse metrology rely on non-linear processes, induced solely by the exciting/probing pulses or the pulses to be characterized. Extension of these approaches to the extreme-ultraviolet (XUV) spectra
l region opens up a new, direct route to attosecond scale dynamics. Limitations in available intensities of coherent XUV continua kept this prospect barren. The present work overcomes this barrier. Reaching condition at which simultaneous ejection of two bound electrons by two-XUV-photon absorption becomes more efficient than their one-by-one removal it is succeeded to probe atomic coherences, evolving at the 1fs scale, and determine the XUV-pulse duration. The investigated rich and dense in structure autoionizing manifold ascertains applicability of the approach to complex systems. This initiates the era of XUV-pump-XUV-probe experiments with attosecond resolution.
The emission of above-ionization-threshold harmonics results from the recombination of two electron wavepackets moving along a short and a long trajectory in the atomic continuum. Attosecond pulse train generation has so far been attributed to the sh
ort trajectory, attempted to be isolated through targeted trajectory-selective phase matching conditions. Here, we provide experimental evidence for the contribution of both trajectories to the harmonic emission, even under phase matching conditions unfavorable for the long trajectory. This is finger printed in the interference modulation of the harmonic yield as a function of the driving laser intensity. The effect is also observable in the sidebands yield resulting from the frequency mixing of the harmonics and the driving laser field, an effect with consequences in cross-correlation pulse metrology approaches.
The two basic approaches underlying the metrology of attosecond pulse trains are compared, i.e. the 2nd order Intensity Volume Autocorrelation and the Resolution of Attosecond Beating by Interference of Two photon Transitions (RABITT). They give rath
er dissimilar results with respect to the measured pulse durations. It is concluded that RABITT may underestimate the duration due to variations of the driving intensity, but in conjunction with theory, allows an estimation of the relative contributions of two different electron trajectories to the extreme-ultraviolet emission.
